Data from observations made at the The Cape Verde Atmospheric Observatory (16.848N, 24.871W) which exists to advance understanding of climatically significant interactions between the atmosphere and ocean and to provide a regional focal point and long-term data. The observatory is based on Calhau Island of São Vicente, Cape Verde in the tropical Eastern North Atlantic Ocean, a region which is data poor but plays a key role in atmosphere-ocean interactions of climate-related and biogeochemical parameters including greenhouse gases. It is an open-ocean site that is representative of a region likely to be sensitive to future climate change, and is minimally influenced by local effects and intermittent continental pollution. The dataset contains mixing ratio measurements of OH and HO2 from University of Leeds during the SOLAS-RHAMBLE intensive measurement campaign.